本文選題：鋯添加劑　切入點(diǎn)：鐵鈰脫硫劑　出處：《太原理工大學(xué)》2017年碩士論文　論文類型：學(xué)位論文

【摘要】：根據(jù)對能源結(jié)構(gòu)和能源消耗的預(yù)測,煤炭將長期占據(jù)我國能源消費(fèi)的主導(dǎo)地位。但隨之而來的是現(xiàn)階段煤炭的低效利用造成了嚴(yán)重的環(huán)境和能源問題。煤的潔凈高效轉(zhuǎn)化技術(shù)將成為解決這一問題的有效途徑。整體煤氣化聯(lián)合循環(huán)(IGCC)和煤基多聯(lián)產(chǎn)(CPG)等發(fā)電技術(shù),以其高效率、低污染的環(huán)境友好特性,成為未來極具潛力的潔凈煤技術(shù)可持續(xù)戰(zhàn)略發(fā)展方向。然而,煤氣化過程中產(chǎn)生的H2S會對管道設(shè)備、環(huán)境及人類健康等方面造成嚴(yán)重的危害。因此,高溫煤氣脫硫技術(shù)的研究具有重要的意義。本論文總結(jié)并分析了鐵鈰復(fù)合基高溫煤氣脫硫劑的優(yōu)勢及存在的問題,選擇以第三組分鋯作為添加劑,制備出具有脫硫活性好的鐵鈰鋯復(fù)合高溫煤氣脫硫劑。在固定床微分反應(yīng)器上考察了鐵鈰鋯復(fù)合脫硫劑的脫硫行為,并結(jié)合XRD、N2吸附、XPS、H2-TPR、SEM-EDS等表征手段,探究鋯添加劑對鐵鈰復(fù)合基脫硫劑結(jié)構(gòu)、還原性能及硫化性能的影響,彼此關(guān)聯(lián),得到以下主要結(jié)論:(1)以共沉淀法制得的鐵鈰鋯復(fù)合脫硫劑,其存在形式為Fe2O3-Ce1-xZrxO2。最佳制備條件為:Fe、Ce、Zr的摩爾比為1:0.8:0.2,焙燒溫度為700oC。鋯添加劑提高了氧化鐵、氧化鈰及鐵鈰復(fù)合脫硫劑的比表面積和孔容,有利于吸脫附硫;鋯添加劑增加了氧化鈰和鐵鈰復(fù)合脫硫劑的氧空位,促進(jìn)了脫硫劑Ce4+→Ce3+的還原。(2)鋯添加劑提高了鐵鈰復(fù)合脫硫劑中Ce4+的還原度,且降低了Ce4+體相還原溫度,有利于脫硫劑中鐵鈰活性組分在相同溫區(qū)進(jìn)行還原反應(yīng)。(3)與單一氧化鐵和氧化鈰脫硫劑相比,當(dāng)硫化溫度為600oC時,鐵鈰復(fù)合脫硫劑表現(xiàn)出更好的硫化性能,但其反應(yīng)程度較低。在此溫度下,鐵鈰復(fù)合脫硫劑中鈰活性組分并未充分參與反應(yīng)。(4)鋯添加劑顯著提高了鐵鈰復(fù)合基脫硫劑的脫硫精度、硫化反應(yīng)活性組分利用率、穿透硫容、硫化反應(yīng)程度并拓寬了其硫化反應(yīng)溫度范圍。對于顆粒脫硫劑而言,還原及硫化反應(yīng)均為由外而內(nèi)的層式反應(yīng)。在還原過程中鋯添加劑促使Ce逐漸向外層富集或Fe逐漸向內(nèi)層遷移,在硫化過程中Ce逐漸向內(nèi)層遷移或Fe逐漸向外層富集,這種Fe、Ce元素的遷移規(guī)律有利于促使Ce參與到還原及硫化反應(yīng)中。鐵鈰鋯脫硫劑的硫化反應(yīng)式為:Fe(7)(8)Zr2CesO(7)(8)(7)(8)3Hg2HsO(7)g(8)(7)(8)Ces2Fe SSO(7)(8)5HsSZr(7)gO(8)222xx)2(1222Xx132(10)(10)(28)(10)(10)(10)--(5)鐵鈰鋯復(fù)合脫硫劑具有良好的硫化/再生循環(huán)穩(wěn)定性。
[Abstract]:Based on projections of energy structure and energy consumption, Coal will occupy the leading position of energy consumption in our country for a long time. However, the low efficiency of coal utilization has caused serious environmental and energy problems at the present stage. The clean and efficient conversion technology of coal will become the solution to this problem. Effective ways. Integrated coal gasification combined cycle (IGCC) and coal-based multi-generation (CPG) and other power generation technologies, Due to its high efficiency and low pollution, environmental friendliness has become a potential sustainable strategic direction for clean coal technology in the future. However, H2S produced in coal gasification process will affect pipeline equipment. Therefore, the study of high temperature gas desulfurization technology is of great significance. This paper summarizes and analyzes the advantages and problems of iron and cerium based high temperature gas desulfurizer. Using the third component of zirconium as the additive, the desulphurizing agent of iron cerium zirconium composite high temperature gas with good desulfurization activity was prepared. The desulphurization behavior of the iron cerium zirconium composite desulfurizer was investigated in a fixed bed differential reactor. The influence of zirconium additive on the structure, reductive property and vulcanization property of iron-cerium composite desulfurizer was investigated by means of XRDD-N _ 2 adsorption and XRDN _ 2 / TPR-SEM-EDS. The main conclusions are as follows: (1) the iron-cerium zirconium composite desulfurizer was prepared by co-precipitation method. The optimum preparation conditions are as follows: the molar ratio of Fe _ 2O _ 3-Ce1-xZrxO _ 2 is 1: 0.8: 0.2, the calcination temperature is 700oC. The zirconium additive increases the specific surface area and pore volume of Fe _ 2O _ 3, ce _ 2O _ 3 and iron-cerium complex desulfurizer, which is beneficial to the adsorption and desorption of sulfur. The addition of zirconium increased the oxygen vacancy of cerium oxide and iron-cerium composite desulfurizer and promoted the desulfurization agent Ce4. 鈫扵he addition of zirconium to Ce3 increased the degree of reduction of Ce4 in iron-cerium complex desulfurizer and reduced the reduction temperature of Ce4 bulk phase. It is favorable to the reduction of iron-cerium active component in desulfurizer at the same temperature. (3) compared with the single iron oxide and cerium oxide desulfurizer, the iron-cerium composite desulfurizer exhibits better vulcanization performance when the curing temperature is 600oC. But the reaction degree is low. At this temperature, the active component of cerium in the iron-cerium compound desulfurization agent does not fully participate in the reaction. The zirconium additive significantly improves the desulphurization precision of the iron-cerium composite desulfurization agent, the utilization ratio of the active component of the sulfidation reaction, and the penetration sulfur capacity. The degree of vulcanization reaction and the temperature range of vulcanization reaction were widened. In the process of reduction, zirconium additive promoted the enrichment of ce towards the outer layer or the migration of Fe to the inner layer, and the ce gradually migrated to the inner layer or Fe to the outer layer during the vulcanization. The migration rule of Fe ~ (2 +) ce is beneficial to promote ce to participate in reduction and vulcanization. The sulfidation reaction formula of iron-cerium zirconium desulphurizer is Fe: Fe _ 7H _ 2H _ sO _ (7) H _ (2) H _ (se) O _ (7) O _ (8) H _ (2) H _ (2) H _ (se) O _ (7) C _ (8) C _ (2) H _ (2) Fe _ (2) O _ (7) SSOO _ (7O) _ (8) HsSZr _ (7) O _ (8222x) ~ (2) C _ (2) O _ (2) O _ (2) (Fe ~ (2 +)) Zirconium complex Desulfurizer has good stability of sulfidation / regeneration cycle.
【學(xué)位授予單位】：太原理工大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：TQ546.5

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